Laboratory-Based Correlative Soft X-ray and Fluorescence Microscopy in an Integrated Setup.

Correlative microscopy is a powerful technique that combines the advantages of multiple imaging modalities to achieve a comprehensive understanding of investigated samples. For example, fluorescence microscopy provides unique functional contrast by imaging only specifically labeled components, especially in biological samples. However, the achievable structural information on the sample in its full complexity is limited. Here, the intrinsic label-free carbon contrast of water window soft X-ray microscopy can complement fluorescence images in a correlative approach ultimately combining nanoscale structural resolution with functional contrast. However, soft X-ray microscopes are complex and elaborate, and are usually installed on large-scale synchrotron radiation sources due to the demanding photon flux requirements. Yet, with modern high-power lasers it has become possible to generate sufficient photon flux from laser-produced plasmas, thus enabling laboratory-based setups. Here, we present a compact table-top soft X-ray microscope with an integrated epifluorescence modality for "in situ" correlative imaging. Samples remain in place when switching between modalities, ensuring identical measurement conditions and avoiding sample alteration or destruction. We demonstrate our new method by multimodal images of several exemplary samples ranging from nanoparticles to various multicolor labeled cell types. A structural resolution of down to 50 nm was reached.

Gouy phase of Bessel-Gaussian beams: theory vs. experiment.

It is well-known that the wave of a freely propagating Gaussian beam experiences an additional π phase shift compared to a plane wave. This phase shift, known as the Gouy phase, has significant consequences in, e.g., nonlinear optics, since the nonlinear processes require high peak intensity and phase matching of the focused beams. Hence, determining and controlling the Gouy phase is crucial in many fields of modern optics and photonics. Here, we develop an analytical model for the Gouy phase of long-range Bessel-Gaussian beams obtained by annihilating highly charged optical vortices. The model accounts for the influence of the relevant experimental parameters (topological charge, radius-to-width ratio of the initial ring-shaped beam, and focal length of the Fourier-transforming lens). We find an evolution of the Gouy phase varying nearly linearly with propagation distance and confirm this result experimentally.

Carrier envelope phase sensitivity of photoelectron circular dichroism.

We report on a combined experimental and numerical study of photoelectron circular dichroism (PECD) induced by intense few-cycle laser pulses, using methyloxirane as the molecular example. Our experiments reveal a remarkably pronounced sensitivity of the PECD strength of double-ionization on the carrier-envelope phase (CEP) of the laser pulses. By comparison to the simulations, which reproduce the measured CEP-dependence for specific orientations of the molecules in the lab frame, we attribute the origin of the observed CEP-dependence of PECD to the CEP-induced modulation of ionization from different areas of the wave functions of three dominant orbitals.

Broadband soft X-ray source from a clustered gas target dedicated to high-resolution XCT and X-ray absorption spectroscopy.

The development of the broad-bandwidth photon sources emitting in the soft X-ray range has attracted great attention for a long time due to the possible applications in high-resolution spectroscopy, nano-metrology, and material sciences. A high photon flux accompanied by a broad, smooth spectrum is favored for the applications such as near-edge X-ray absorption fine structure (NEXAFS), extended X-ray absorption fine structure (EXAFS), or XUV/X-ray coherence tomography (XCT). So far, either large-scale facilities or technologically challenging systems providing only limited photon flux in a single shot dominate the suitable sources. Here, we present a soft, broad-band (1.5 nm - 10.7 nm) soft X-ray source. The source is based on the interaction of very intense laser pulses with a target formed by a cluster mixture. A photon yield of 2.4 × 1014 photons/pulse into 4π (full space) was achieved with a medium containing Xe clusters of moderate-size mixed with a substantial amount of extremely large ones. It is shown that such a cluster mixture enhances the photon yield in the soft X-ray range by roughly one order of magnitude. The size of the resulting source is not beneficial (≤500 µm but this deficit is compensated by a specific spectral structure of its emission fulfilling the specific needs of the spectroscopic (broad spectrum and high signal dynamics) and metrological applications (broad and smoothed spectrum enabling a sub-nanometer resolution limit for XCT).

Absolute EUV reflectivity measurements using a broadband high-harmonic source and an in situ single exposure reference scheme.

We present a tabletop setup for extreme ultraviolet (EUV) reflection spectroscopy in the spectral range from 40 to 100 eV by using high-harmonic radiation. The simultaneous measurements of reference and sample spectra with high energy resolution provide precise and robust absolute reflectivity measurements, even when operating with spectrally fluctuating EUV sources. The stability and sensitivity of EUV reflectivity measurements are crucial factors for many applications in attosecond science, EUV spectroscopy, and nano-scale tomography. We show that the accuracy and stability of our in situ referencing scheme are almost one order of magnitude better in comparison to subsequent reference measurements. We demonstrate the performance of the setup by reflective near-edge x-ray absorption fine structure measurements of the aluminum L2/3 absorption edge in α-Al2O3 and compare the results to synchrotron measurements.

Characterization of encapsulated graphene layers using extreme ultraviolet coherence tomography.

Many applications of two-dimensional materials such as graphene require the encapsulation in bulk material. While a variety of methods exist for the structural and functional characterization of uncovered 2D materials, there is a need for methods that image encapsulated 2D materials as well as the surrounding matter. In this work, we use extreme ultraviolet coherence tomography to image graphene flakes buried beneath 200 nm of silicon. We show that we can identify mono-, bi-, and trilayers of graphene and quantify the thickness of the silicon bulk on top by measuring the depth-resolved reflectivity. Furthermore, we estimate the quality of the graphene interface by incorporating a model that includes the interface roughness. These results are verified by atomic force microscopy and prove that extreme ultraviolet coherence tomography is a suitable tool for imaging 2D materials embedded in bulk materials.

Carrier-envelope phase stable few-cycle laser system delivering more than 100 W, 1 mJ, sub-2-cycle pulses.

Two-stage multipass-cell compression of a fiber-chirped-pulse amplifier system to the few-cycle regime is presented. The output delivers a sub-2-cycle (5.8 fs), 107 W average power, 1.07 mJ pulses at 100 kHz centered at 1030 nm with excellent spatial beam quality (M2 = 1.1, Strehl ratio S = 0.98), pointing stability (2.3 µrad), and superior long-term average power stability of 0.1% STD over more than 8 hours. This is combined with a carrier-envelope phase stability of 360 mrad in the frequency range from 10 Hz to 50 kHz, i.e., measured on a single-shot basis. This unique system will serve as an HR1 laser for the Extreme Light Infrastructure Attosecond Light Pulse Source research facility to enable high repetition rate isolated attosecond pulse generation.

Laser-Driven Anharmonic Oscillator: Ground-State Dissociation of the Helium Hydride Molecular Ion by Midinfrared Pulses.

The vibrational motion of molecules represents a fundamental example of an anharmonic oscillator. Using a prototype molecular system, HeH^{+}, we demonstrate that appropriate laser pulses make it possible to drive the nuclear motion in the anharmonic potential of the electronic ground state, increasing its energy above the potential barrier and facilitating dissociation by purely vibrational excitation. We find excellent agreement between the frequency-dependent response of the helium hydride molecular cation to both classical and quantum mechanical simulations, thus removing any ambiguities through electronic excitation. Our results provide access to the rich dynamics of anharmonic quantum oscillator systems and pave the way to state-selective control schemes in ground-state chemistry by the adequate choice of the laser parameters.

Long-range quasi-non-diffracting Gauss-Bessel beams in a few-cycle laser field.

Many applications ranging from nonlinear optics to material processing would benefit from pulsed ultrashort (quasi-)non-diffracting Gauss-Bessel beams (GBBs). Here we demonstrate a straightforward yet efficient method for generating such zeroth- and first-order GBBs using a single reflective spatial light modulator. Even in the sub-8-fs range there are no noticeable consequences for the measured pulse duration. The only effect is a weak "coloring" of the outer-lying satellite rings of the beams due to the spectrum spanning over more than 300 nm. The obtained beams have diffraction half-angles below 40 µrad and reach propagation distances in excess of 1.5 m.

Advanced X-ray polarimeter design for nuclear resonant scattering.

This work presents the improvements in the design and testing of polarimeters based on channel-cut crystals for nuclear resonant scattering experiments at the 14.4 keV resonance of 57Fe. By using four asymmetric reflections at asymmetry angles of α1 = -28°, α2 = 28°, α3 = -28° and α4 = 28°, the degree of polarization purity could be improved to 2.2 × 10-9. For users, an advanced polarimeter without beam offset is now available at beamline P01 of the storage ring PETRA III.

Zeroth- and first-order long range non-diffracting Gauss-Bessel beams generated by annihilating multiple-charged optical vortices.

We demonstrate an alternative approach for generating zeroth- and first-order long range non-diffracting Gauss-Bessel beams (GBBs). Starting from a Gaussian beam, the key point is the creation of a bright ring-shaped beam with a large radius-to-width ratio, which is subsequently Fourier-transformed by a thin lens. The phase profile required for creating zeroth-order GBBs is flat and helical for first-order GBBs with unit topological charge (TC). Both the ring-shaped beam and the required phase profile can be realized by creating highly charged optical vortices by a spatial light modulator and annihilating them by using a second modulator of the same type. The generated long-range GBBs are proven to have negligible transverse evolution up to 2 m and can be regarded as non-diffracting. The influences of the charge state of the TCs, the propagation distance behind the focusing lens, and the GBB profiles on the relative intensities of the peak/rings are discussed. The method is much more efficient as compared to this using annular slits in the back focal plane of lenses. Moreover, at large propagation distances the quality of the generated GBBs significantly surpasses this of GBBs created by low angle axicons. The developed analytical model reproduces the experimental data. The presented method is flexible, easily realizable by using a spatial light modulator, does not require any special optical elements and, thus, is accessible in many laboratories.

Carrier-envelope-phase measurement of few-cycle mid-infrared laser pulses using high harmonic generation in ZnO.

High-harmonic generation (HHG) in crystals offers a simple, affordable and easily accessible route to carrier-envelope phase (CEP) measurements, which scales favorably towards longer wavelengths. We present measurements of HHG in ZnO using few-cycle pulses at 3.1µm. Thanks to the broad bandwidth of the driving laser pulses, spectral overlap between adjacent harmonic orders is achieved. The resulting spectral interference pattern provides access to the relative harmonic phase, and hence, the CEP.

Observing the Importance of the Phase-Volume Effect for Few-Cycle Light-Matter Interactions.

The spatially dependent phase distribution of focused few-cycle pulses, i.e., the focal phase, is much more complex than the well-known Gouy phase of monochromatic beams. As the focal phase is imprinted on the carrier-envelope phase (CEP), for accurate modeling and interpretation of CEP-dependent few-cycle laser-matter interactions, both the coupled spatially dependent phase and intensity distributions must be taken into account. In this Letter, we demonstrate the significance of the focal phase effect via comparison of measurements and simulations of CEP-dependent photoelectron spectra. Moreover, we demonstrate the impact of this effect on few-cycle light-matter interactions as a function of their nonlinear intensity dependence to answer the general question: if, when, and how much should one be concerned about the focal phase?

Experimental Separation of Subcycle Ionization Bursts in Strong-Field Double Ionization of H_{2}.

We report on the unambiguous observation of the subcycle ionization bursts in sequential strong-field double ionization of H_{2} and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase, in combination with multiparticle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state-specific Coulomb distortions on emitted electrons in polyatomic molecules.

Absolute carrier-envelope-phase dependences of single and double ionization of methanol in a near-IR few-cycle laser field.

We investigate the carrier-envelope phase (CEP) dependences of the single and double ionization processes of methanol (CH3OH) in an intense near-IR few-cycle laser field (2.1 × 1014 W/cm2) by the asymmetry in the ejection direction of CH3 + for the non-hydrogen migration channels and CH2 + for the hydrogen migration channels created through the C-O bond breaking after the ionization. Based on the absolute CEP values at the laser-molecule interaction point, calibrated by the method using intense few-cycle circularly polarized laser pulses [Fukahori et al., Phys. Rev. A 95, 053410-1-053410-14 (2017)], we confirm that methanol cations are produced by tunnel ionization and methanol dications are produced by the recollisional double ionization. We obtain the phase offset for the double ionization accompanying no hydrogen migration to be 1.85π as the absolute CEP at which the extent of the asymmetry becomes maximum. We interpret the phase shift of 0.85π from the phase offset of 1.0π for the tunnel ionization, estimated by a tunnel ionization model incorporating the chemical bond asymmetry, as the corresponding time delay associated with the electron recollisional ionization. The positive phase shift of 0.13π for the single ionization in the non-hydrogen migration channel is interpreted as the additional time (165 as) with which a methanol cation can be excited electronically prior to the decomposition. The additional phase shift of 0.22π for the single ionization in the hydrogen migration channel is interpreted as the additional time (280 as) required for a methanol cation to be excited electronically leading to the hydrogen migration prior to the decomposition.

Laboratory setup for extreme ultraviolet coherence tomography driven by a high-harmonic source.

We present a laboratory beamline dedicated to nanoscale subsurface imaging using extreme ultraviolet coherence tomography (XCT). In this setup, broad-bandwidth extreme ultraviolet (XUV) radiation is generated by a laser-driven high-harmonic source. The beamline is able to handle a spectral range of 30-130 eV and a beam divergence of 10 mrad (full width at half maximum). The XUV radiation is focused on the sample under investigation, and the broadband reflectivity is measured using an XUV spectrometer. For the given spectral window, the XCT beamline is particularly suited to investigate silicon-based nanostructured samples. Cross-sectional imaging of layered nanometer-scale samples can be routinely performed using the laboratory-scale XCT beamline. A depth resolution of 16 nm has been achieved using the spectral range of 36-98 eV which represents a 33% increase in resolution due to the broader spectral range compared to previous work.

A high resolution extreme ultraviolet spectrometer system optimized for harmonic spectroscopy and XUV beam analysis.

We present a modular extreme ultraviolet (XUV) spectrometer system optimized for a broad spectral range of 12-41 nm (30-99 eV) with a high spectral resolution of λ/Δλ ≳ 784 ± 89. The spectrometer system has several operation modes for (1) XUV beam inspection, (2) angular spectral analysis, and (3) imaging spectroscopy. These options allow for a versatile use in high harmonic spectroscopy and XUV beam analysis. The high performance of the spectrometer is demonstrated using a novel cross-sectional imaging method called XUV coherence tomography.

Subfemtosecond Tracing of Molecular Dynamics during Strong-Field Interaction.

We introduce and experimentally demonstrate a method where the two intrinsic timescales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photoelectron photoion coincidence experiment. In our experiment, elliptically polarized, 750 nm, 4.5 fs laser pulses were focused to an intensity of 9×10^{14} W/cm^{2} onto H_{2}. Using coincidence imaging, we directly observe the nuclear wave packet evolving on the 1sσ_{g} state of H_{2}^{+} during its first round-trip with attosecond temporal and picometer spatial resolution. The demonstrated method should enable insight into the first few femtoseconds of the vibronic dynamics of ionization-induced unimolecular reactions of larger molecules.

Heteronuclear Limit of Strong-Field Ionization: Fragmentation of HeH

The laser-induced fragmentation dynamics of this most fundamental polar molecule HeH^{+} are measured using an ion beam of helium hydride and an isotopologue at various wavelengths and intensities. In contrast to the prevailing interpretation of strong-field fragmentation, in which stretching of the molecule results primarily from laser-induced electronic excitation, experiment and theory for nonionizing dissociation, single ionization, and double ionization both show that the direct vibrational excitation plays the decisive role here. We are able to reconstruct fragmentation pathways and determine the times at which each ionization step occurs as well as the bond length evolution before the electron removal. The dynamics of this extremely asymmetric molecule contrast the well-known symmetric systems leading to a more general picture of strong-field molecular dynamics and facilitating interpolation to systems between the two extreme cases.

Continuous every-single-shot carrier-envelope phase measurement and control at 100 kHz.

With the emergence of high-repetition-rate few-cycle laser pulse amplifiers aimed at investigating ultrafast dynamics in atomic, molecular, and solid-state science, the need for ever faster carrier-envelope phase (CEP) detection and control has arisen. Here we demonstrate a high-speed, continuous, every-single-shot measurement and fast feedback scheme based on a stereo above-threshold ionization time-of-flight spectrometer capable of detecting the CEP and pulse duration at a repetition rate of up to 400 kHz. This scheme is applied to a 100 kHz optical parametric chirped pulse amplification few-cycle laser system, demonstrating improved CEP stabilization and allowing for CEP tagging.